The performance of a lithium metal anode was studied in a poly(vinylidene fluoride-hexafluoropropylene) (PVdF-HFP) gel electrolyte. By using the PVdF-HFP gel electrolyte, we obtained a higher coulombic efficiency (ca. 85%) and a more uniform morphology of the lithium metal anode than those obtained with the propylene carbonate liquid or the poly(ethylene oxide) gel system. Additionally, the CO 2 addition to the PVdF-HFP gel system improved both the the uniformity in morphology of the lithium anode and the coulombic efficiency further to ca. 95%.The gel electrolyte, which consists of polymer matrix, organic solvent, and supporting electrolyte, was introduced as a novel material in the field of rechargeable battery applications as early as 1975. 1-3 Two advantages of the gel electrolyte applied to batteries include the fact that the electrolyte solution does not leak out from the cell, and that the electrolyte can be prepared as a thin film, which allows construction of a solid-state and high energy density battery. In particular, the gel electrolyte demonstrates a high ionic conductivity of about 10 -3 S cm -1 at room temperature and has a sufficient mechanical strength. Examples of the host polymer of the gel electrolyte are poly(acrylonitrile), 4,5 poly(methylmethacrylate), 3,4 and a new copolymer of vinylidene fluoride with hexafluoropropylene (PVdF-HFP). 6-9 The first reliable and practical rechargeable Li-ion plastic battery, which contained the carbon material as the anode, was developed in 1996 using the PVdF-HFP copolymer-type gel electrolyte. 10 For the next generation of rechargeable batteries, the lithium secondary battery using lithium metal as the anode is the most attractive candidate for higher energy power sources for portable electronic devices, electric vehicles, and load-leveling systems. Lithium metal demonstrates a remarkably low electrochemical equivalent and the most negative redox potential of all the metallic elements. There are, however, some disadvantages of the lithium metal anode compared to the carbon anode. The charge-discharge cycle life of the lithium metal anode is degraded by the formation of dendritic deposits, which causes the isolation of active lithium metal and also leads to short circuit with the cathode. Another reason for the poor cycle life of the lithium anode may be the formation of an interfacial layer between lithium metal and electrolyte with a low ionic or electronic conductivity as discussed in Ref. 9 and 10.In order to improve the lithium anode properties, the effect of additives to the liquid electrolyte was studied, e.g., CO 2 11-15 and HF. 16,17 Recently, we confirmed that a poly(ethylene oxide) (PEO) -based gel electrolyte effectively suppressed the dendritic deposition of lithium. 18 In the present study, the excellent charge-discharge performance of the lithium metal anode obtained with the PVdF-HFP gel electrolyte system is demonstrated. Furthermore, the effect of CO 2 addition to the PVdF-HFP gel electrolyte was investigated.Experimental The details of th...